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Mn Doping Induced Ordering Transformation and Strain Engineering in a PtCu Alloy for Enhanced Oxygen Reduction
Xue Zhang1, Hao Sun1, Yuanhua Sun1
1School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China.
None:
Developing active and durable platinum-based catalysts is critical for advancing proton-exchange membrane fuel cells (PEMFCs). To overcome the Cu dissolution and poor stability of PtCu intermetallics, we propose a Mn-doping strategy to fabricate L10-ordered PtCuMn nanocatalysts. Mn incorporation modulates the Pt electronic structure, enhances L10 ordering, and induces compressive strain within a Pt-rich shell. Consequently, the catalyst demonstrates exceptional oxygen reduction reaction (ORR) activity with a half-wave potential of 0.921 V, a mass activity (MA) of 0.96 A mgPt-1 and a negligible half-wave potential shift after 30 000 cycles. In PEMFCs, it delivers peak power densities of 1.31 W cm-2 (H2-air) and 2.23 W cm-2 (H2-O2). Furthermore, its MA reaches 0.78 A mgPt-1, which exceeds the U.S. Department of Energy (DOE) 2025 target. Operando characterizations and theoretical calculations confirm that Mn doping downshifts the Pt d-band center, accelerates the conversion kinetics of the key *OH intermediate, and thereby optimizes the ORR performance.
